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The Sierra de San Luis constitutes the southernmost tip of the Eastern Sierras Pampeanas. Its Palaeozoic metamorphic basement units define a key location for the understanding of the accretional history along the proto-Andean margin of Gondwana. Although, it is largely accepted that the polyphase accretional history of the Sierras Pampeanas is preluded by the docking of the Pampean Terrane followed by the Famatinian Orogenic Cycle that involves subduction along the margin of Gondwana and the accretion of the Precordillera (Cuyania) Terrane and finally ceased with the collision of the Chilenia terrane, a vast amount of controversial information concerning the timing and mode of collisions as well as the origin of the different involved crustal fragments within the Eastern Sierras Pampeanas is published. In this paper, those different hypothesis are presented and evaluated under the light of new isotopic data of the Sierra de San Luis. Nd-systematics of the metasedimentary sequences of the Sierra de San Luis indicate that the studied sequences were developed on the Pampean Terrane. An Amazonian origin of the Pampean Terrane that was probably detached from the Arequipa Antofalla Craton is proposed. Furthermore, the correlation of two low-grade phyllitic belts (San Luis Formation) with the widespread Puncoviscana Formation is not supported by Sm-Nd data. It is suggested that the sedimentary precursors of the Pringles Metamorphic Complex and the topping phyllites were sourced on the Pampean Orogen and accommodated in a newly formed back arc basin during the early Famatinian. The cooling history of the basement complex is recorded by an extensive amount of K-Ar muscovite and biotite ages. A high variability in muscovite ages is only partly related to different intrusion times of two pegmatoid generations. Post Famatinian to Achalian crustal scale mylonite formation (-359 Ma) and a rotational exhumation of the central basement unit are causal for the observed K-Ar muscovite age pattern in the range from 395 Ma to 447 Ma. Therefore, the decrease in metamorphic degree from west to east is the result of the erosion level of a crustal profile from the mid lower crust to the upper crust. An even higher variability in K-Ar biotite cooling ages covering the range from 315 Ma to 418 Ma is related to the slow cooling after the Famatinian Orogenic Cycle or reheating during the Achalian Orogenic Cycle and consequent variable reset of the isotopic system. However, ages recorded by biotite booklets substantiate the hypothesis of a differential exhumation of the basement of the Sierra de San Luis.